Validation and investigation of reactive species yields of Geant4‐ DNA chemistry models

Dylan Peukert (1) , Sebastien Incerti (2) , Ivan Kempson (1) , Michael Douglass (3, 4, 5) , Mathieu Karamitros (6) , Gérard Baldacchino (7, 8) , Eva Bezak (4)

1 University of South Australia [Adelaide]
2 CENBG - Centre d'Etudes Nucléaires de Bordeaux Gradignan
3 Royal Adelaide Hospital [Adelaide Australia]
4 University of Adelaide
5 Department of Physics and Mathematical Physics [Adelaide]
6 UND - University of Notre Dame [Indiana]
7 DICO - Dynamique et Interactions en phase Condensée
8 LIDYL - Laboratoire Interactions, Dynamiques et Lasers (ex SPAM)

Purpose: Indirect biological damage due to reactive species produced in water radiolysis reactions is responsible for the majority of biological effect for low linear energy transfer (LET) radiation. Modeling water radiolysis and the subsequent interactions of reactive species, as well as track structures, is essential to model radiobiology on the microscale. Recently, chemistry models have been developed for Geant4-DNA to be used in combination with the comprehensive existing physics models. In the current work, the first detailed, independent, in silico validation of all species yields with published experimental observations and comparison with other radiobiological simulations is presented. Additionally, the effect of LET of protons and heavier ions on reactive species yield in the model was examined, as well as the completeness of the chemical reactions following the radiolysis within the time after physical interactions simulated in the model. Methods: Yields over time of reactive species were simulated for water radiolysis by incident electrons, protons, alpha particles, and ions with various LETs using Geant4 and RITRACKS simulation tools. Water dissociation and recombination was simulated using Geant4 to determine the completeness of chemical reactions at the end of the simulation. Yield validation was performed by comparing yields simulated using Geant4 with experimental observations and other simulations. Validation was performed for all species for low LET radiation and the solvated electron and hydroxyl radical for high LET ions. Results: It was found that the Geant4-DNA chemistry yields were generally in good agreement with experimental observations and other simulations. However, the Geant4-DNA yields for the hydroxyl radical and hydrogen peroxide at the end of the chemistry stage were found to be respectively considerably higher and lower than the experimentally observed yields. Increasing the LET of incident hadrons increased the yield of secondary species and decreased the yield of primary species. The effect of LET on the yield of the hydroxyl radical at 100 ns simulated with Geant4 was in good agreement with experimental measurements. Additionally, by the end of the simulation only 40% of dissociated water molecules had been recombined and the rate of recombination was slowing. Conclusions: The yields simulated using Geant4 are within reasonable agreement with experimental observations. Higher LET radiation corresponds with increased yields of secondary species and decreased yields of primary species. These trends combined with the LET having similar effects on the 100 ns hydroxyl radical yield for Geant4 and experimental measurements indicate that Geant4 accurately models the effect of LET on radiolysis yields. The limited recombination within the modeled chemistry stage and the slowing rate of recombination at the end of the stage indicate potential long-range indirect biological damage.

Mots clés: model validation; radiation chemistry; radiobiology; water radiolysis; Monte Carlo

Domaines: Chimie théorique et/ou physique; Chimie-Physique [physics.chem-ph]

Dylan Peukert, Sebastien Incerti, Ivan Kempson, Michael Douglass, Mathieu Karamitros, et al.. Validation and investigation of reactive species yields of Geant4‐ DNA chemistry models. Medical Physics, 2019, 46 (2), pp.983-998. ⟨10.1002/mp.13332⟩. ⟨cea-01978196⟩